A DFT and KMC based study on the mechanism of the water gas shift reaction on the Pd(100) surface

Chutia, Arunabhiram, Thetford, Adam, Stamatakis, Michail and Catlow, C. Richard A. ORCID: https://orcid.org/0000-0002-1341-1541 2020. A DFT and KMC based study on the mechanism of the water gas shift reaction on the Pd(100) surface. Physical Chemistry Chemical Physics 22 (6) , pp. 3620-3632. 10.1039/C9CP05476F

Preview

PDF - Accepted Post-Print Version Download (1MB) | Preview

Abstract

We present a combined density functional theory (DFT) and Kinetic Monte Carlo (KMC) study of the water gas shift (WGS) reaction on the Pd(100) surface. We propose a mechanism comprising both the redox and the associative pathways for the WGS within a single framework, which consists of seven core elementary steps, which in turn involve splitting of a water molecule followed by the production of an H-atom and an OH-species on the Pd(100) surface. In the following steps, these intermediates then recombine with each other and with CO leading to the evolution of CO2, and H2. Seven other elementary steps, involving the diffusion and adsorption of the surface intermediate species are also considered for a complete description of the mechanism. The geometrical and electronic properties of each of the reactants, products, and the transition states of the core elementary steps are presented. We also discuss the analysis of Bader charges and spin densities for the reactants, transition states and the products of these elementary steps. Our study indicates that the WGS reaction progresses simultaneously via the direct oxidation and the carboxyl paths on the Pd(100) surface.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Advanced Research Computing @ Cardiff (ARCCA) Cardiff Catalysis Institute (CCI) Chemistry
Publisher:	Royal Society of Chemistry
ISSN:	1463-9076
Funders:	EPSRC
Date of First Compliant Deposit:	12 March 2020
Date of Acceptance:	6 January 2020
Last Modified:	08 Nov 2024 21:15
URI:	https://orca.cardiff.ac.uk/id/eprint/130373

Citation Data

Cited 17 times in Scopus. View in Scopus. Powered By Scopus® Data

Actions (repository staff only)

Edit Item